CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Sufeng An,Guanghui Zhang,Jiaqiang Liu,Keyan Li,Gang Wan,Yan Liang,Donghui Ji,Jeffrey T. Miller,Chunshan Song,Wei Liu,Zhongmin Liu,Xinwen Guo
Heterogeneous catalysts with ultra-small clusters and atomically dispersed (USCAD) active sites have gained increasing attention in recent years. However, developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging. Here, through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine (MA), porous alveolate Fe/g-C 3 N 4 catalysts with high-density (Fe loading up to 17.7 wt%) and increased USCAD Fe sites were synthesized. The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts; the S species act as a “sacrificial carrier” to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO 2 during pyrolysis . The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts, due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure. This S-assisted method exhibits good feasibility in a large variety of S species (thiourea, S powder, and NH 4 SCN) and Fe salts, providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C 3 N 4 catalysts.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 33
·19669-19685
·
IF 3.119
Shuting Zhang,Guoqiang Li,Liyuan Duan,Hongyu Wang,Yongle Zhao,Yongfa Zhang
Graphitic carbon nitride (g-C3N4) was prepared by a simple thermal polymerization method in this work. The effects of precursor type, thermal polymerization temperature, constant temperature time and atmosphere on the crystal structure, morphology, elemental composition, valence distribution, light absorption properties and photocatalytic activity of the prepared photocatalytic materials were investigated. Taking rhodamine B (RhB) as the target degradant, the blue light catalytic activity of the photocatalytic material was studied in detail. The experimental results showed that the final pyrolysis temperature and constant temperature time are positively related to the adsorption characteristics and photocatalytic ability of the prepared materials. In addition, the adsorption capacity and photocatalytic activity of the products obtained in Ar and H2 atmospheres are better than those produced in CO and CH4, which can be attributed to the combined effect of large specific surface area and structural defects of the materials. The sample's large specific surface area, wide band gap, and excellent photogenerated carrier separation and transfer capabilities make the adsorption performance and photocatalytic performance of the products obtained with ammonium thiocyanate and thiourea as precursors better than those prepared from melamine and dicyandiamide. g-C3N4 prepared by using ammonium thiocyanate as precursor at 550 °C for 5 h under a hydrogen atmosphere showed the best catalytic activity for the degradation of RhB under blue light. It was demonstrated that g-C3N4 prepared exhibited good stability and reusability after four repeat experiments. The active components that play major roles in the degradation of RhB described herein were holes and superoxide radicals, which was inferred by free radical trapping experiments. This work provides a theoretical basis for the idea of converting the mixed salts of desulfurization waste liquid containing ammonium thiocyanate into an excellent photocatalyst g-C3N4 with visible light response.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS RESEARCH BULLETIN
·
2020
·
IF 4.019
Zhongwei Fan,Jingfei Luan,Changqing Zhu,Fuqiang Liu
The novel Z-scheme heterojunction photocatalyst g-C 3 N 4 /Ag 2 S/SnS 2 with Ag 2 S quantum dots as electron mediators was successfully synthesized by in-situ ion exchange reaction and self-peeling of g-C 3 N 4 . Compared with g-C 3 N 4 , SnS 2 or g-C 3 N 4 /SnS 2 , the photocatalyst g-C 3 N 4 /Ag 2 S/SnS 2 exhibited more excellent photocatalytic performance under visible light irradiation. The removal rate of methyl orange was 96.8% after 30 minutes visible light irradiation and the reaction rate constant reached 0.10225 min -1 . The enhanced photocatalytic activity could be attributed to the formation of Z-scheme heterojunction structure and the 2D layered structure. The electrochemical and photoelectric performance tests showed that the separation and transfer efficiency of the photogenic electron-hole pairs as well as the redox potential were significantly improved. Additionally, the quenching experiments showed that the superoxide radicals and holes were the primarily active species. Combined with other characterizations, the reaction mechanism of the g-C 3 N 4 /Ag 2 S/SnS 2 for degrading the target pollutant methyl orange under visible light irradiation was proposed.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Ping Sun,Hui Liu,Mingbao Feng,Zhicai Zhai,Yingsen Fang,Xuesheng Zhang,Virender K. Sharma
In this study, two metal-free materials, i.e., N-doped graphene (rGO-N) and g-C 3 N 4 , were strategically combined to prepare a novel g-C 3 N 4 /rGO-N composite for activating peroxymonosulfate (PMS). The g-C 3 N 4 /rGO-N composite showed large specific surface area and high graphite-rich N content, and hence, exhibited excellent catalytic performance because of the synergistic effect of g-C 3 N 4 and rGO-N. The oxidative system could effectively degrade various pollutants (e.g., acid orange 7, orange G, ciprofloxacin, and bisphenol A). The radical quenching experiments and electron paramagnetic resonance spectra analysis revealed that the novel carbonaceous composite could realize PMS-based non-radical oxidative degradation of pollutants unlike the previously reported catalysts, observed the degradation via a radical-dominated pathway. The real-time water treatment experiments demonstrated the potential of the oxidative system to environmental remediation applications. The combination strategy provides an innovative approach to fabricate binary metal-free carbonaceous catalysts for carrying out PMS-based non-radical oxidative degradation of pollutants.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Wen Cao,Yuhang Yuan,Cao Yang,Shichuan Wu,Jianhua Cheng
For the first time, visible-light-driven g-C 3 N 4 /MIL-68(In)-NH 2 heterojunction composites with high photocatalytic activity were prepared for the degradation of ibuprofen (IBP) using an in-situ solvothermal synthesis method assisted with ultrasonication. The composites achieved intensive visible-light absorption, enhanced separation efficiency of photogenerated carriers, and high adsorption capacity, thus achieving excellent photocatalytic degradation for IBP. Among all the composites, 10 wt% g-C 3 N 4 /MIL-68(In)-NH 2 exhibited the maximum photocatalytic rate (0.01739 min −1 ), 19.28 and 2.00 times higher than those of g-C 3 N 4 and MIL-68(In)-NH 2 , respectively. Moreover, the pH, ibuprofen concentration, and catalyst dosages played important roles both in photodegradation and adsorption. In addition, the photocatalytic mechanism was also elucidated, demonstrating that h + was the main reactive species, followed by OH and O 2 − radicals, responsible for the degradation of IBP. Finally, seven aromatic intermediates of IBP were identified, and five possible degradation pathways were proposed, mainly involving hydroxylation, aldehyde oxidation, decarboxylation, and dehydrogenization reactions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ruiyang Zhang,Tao Ran,Yuehan Cao,Liqun Ye,Fan Dong,Qian Zhang,Lizhi Yuan,Ying Zhou
Photocatalytic NO x removal is regarded as a promising technique for air purification in recent years. However, NO x removal process usually accompanies with toxic NO 2 generation, leading to serious secondary pollutant and limiting its practical application. Herein, a noble-metal-free g-C 3 N 4 /α-Ni(OH) 2 photocatalyst was fabricated through hydrothermal method. The introduction of α-Ni(OH) 2 microspheres combines with g-C 3 N 4 , resulting in an enlarged surface area from 35 to 95 m 2 /g, while the unique structure of α-Ni(OH) 2 broadens visible-light response range and accelerates photogenerated charge carriers transfer. More importantly, the H atoms of α-Ni(OH) 2 improve the adsorption and activation of O 2 and oxygen atoms to promote NO and NO 2 oxidized to nitrate. Consequently, g-C 3 N 4 /α-Ni(OH) 2 shows enhanced NO removal ratio of 51.3% without any toxic NO 2 generation, indicating its great potential for air purification. Our results provide fresh insight into the design of highly efficient and safe photocatalyst for toxic byproduct control in the application of environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Pengjia Sun,Jian Xiong,Ping Sun,Yingsen Fang,Hongxia Liu,Hui Liu,Bitao Xiong,Hui Wang,Xing'ao Li
Metal-doped g-C 3 N 4 materials have been extensively investigated and utilized as catalysts in the domain of wastewater treatment. In this study, additional O was introduced in Mn-doped g-C 3 N 4 (MCN) to synthesize Mn/O co-doped material (MOCN), and a new non-radical oxidation system of periodate (PI) activation with MOCN was established for degradation of pollutants. The results indicated that additional O doping can enhance the catalytic performance of MOCN. This was primarily demonstrated by the 3.5-fold increase in the degradation rate ( k ) of sulfadiazine (SDZ) by MOCN/PI system compared to MCN/PI one. Simultaneously, density functional theory (DFT) calculations have revealed that MOCN material exhibit a higher affinity for adsorbing PI (adsorption energy E ads = −4.992 eV), resulting in an elongation of the I-O bond length ( l I-O = 1.874 Å) and facilitating bond cleavage of PI to generate reactive active species (ROS). The reaction process was confirmed to be primarily driven by non-radical singlet oxygen ( 1 O 2 ), as demonstrated by electron paramagnetic resonance (EPR) and free radical quenching experiments. In addition, possible degradation pathways of SDZ were proposed based on the identified intermediate products and the calculated Fukui constants. The MOCN/PI catalytic system was highly efficient and environmentally friendly, with great potential for development in sewage treatment.
✓ 已验证
产品关联
DOI
高影响因子
DESALINATION
·
2023
·
IF 9.9
Xueying Gao,Zhenzhen Fu,Yanfei Sun,Dewei Wang,Xiaoxuan Wang,Zishan Hou,Jinrui Wang,Xia Liu,Shiyu Wang,Shuyun Yao,Huiying Zhang,Shuyuan Li,Zheng Tang,Weijie Fu,Kaiqi Nie,Jiangzhou Xie,Zhiyu Yang,Yi-Ming Yan
While MnO 2 has been identified as a potent agent in the desalination process , its efficacy is significantly impeded by its inherent poor electrical conductivity and substantial ion diffusion barriers . By orchestrating an interfacial electron bridge within the MnO 2 /g-C 3 N 4 heterostructure , reinforced through N p z -Mn d z 2 orbital hybridization, we have managed to significantly boost both SAC and SAR in the HCDI process. The reinforced N p z -Mn d z 2 orbital hybridization triggers a substantial electron transition from g-C 3 N 4 to MnO 2 , culminating in a high Mn d z 2 electron occupancy. Further analysis reveals the formation of a Mn N chemical bond at the MnO 2 /g-C 3 N 4 interface, operating as an essential electron transfer bridge from g-C 3 N 4 to MnO 2 . This process concurrently initiates a rise in the Mn d z 2 orbital energy level, equipping the Mn d z 2 electron with superior redox activity. With these enhancements, the manufactured MnO 2 /g-C 3 N 4 exhibits exemplary performance, boasting an improved SAC of 68 mg g −1 and SAR of 3.6 mg g −1 min −1 with a decreased energy consumption of 0.7224 kWh kg −1 at 1.2 V. This innovative work offers an unconventional roadmap for activating electron redox activity and thereby accelerating charge transfer in transition metal oxides .
✓ 已验证
产品关联
DOI
高影响因子
Food Frontiers
·
2023
·Vol. 4
·期 4
·1913-1926
·
IF 9.9
Chun-Yang Li,Lu Yang,Yingshuang Lu,Man-Man Wang,Jing-Min Liu,Shuo Wang
Photocatalysis-based advanced oxidation technologies have been developed as an attractive strategy for degrading pollutants. However, the question of how to increase removal specificity without sacrificing the degradation effect remains a difficult one. In this work, a photocatalytic system for the simultaneous targeted elimination of nine heterocyclic amines (HCAs) is established using a green-prepared photocatalyst (CN@Mn–FeOOH@MIP) that activates sodium persulfate (PS) under visible light. Mn–FeOOH clusters are in situ covered on laminar g-C 3 N 4 (CN) carrier to form a heterojunction, along with a molecularly imprinted layer self-polymerized from dopamine, which is grown on the outer layer, resulting in both the desired photochemical activity and specific sites for recognition. The conditions of composite and photocatalysis are explored and optimized for efficient and selective degradation. Notably, CN@Mn–FeOOH@MIP is synthesized free of any organic reagents, and the biosafety is confirmed by cellular and in vivo toxicity evaluation. The developed CN@Mn–FeOOH@MIP/PS system with visible-light-driven is applied to the removal of HCAs in coffee samples with the recoveries over 70% and the reuse rates greater than 85%. It coupled the advantages of specific enrichment and rapid degradation, which furnishes a novel approach for the control of trace thermal processing pollutants.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 31
·14828-14839
·
IF 3.3
Lin Dong,Yunlan Xu,Dengjie Zhong,Nianbing Zhong,Zhuofan Han,Yi Liu,Haixing Chang
The low electron–hole separation in the photoanode generally restricts the visible light response of photocatalytic fuel cell (PFCs). In this study, 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode was synthesized and assembled with a PFC with Cu cathode to degrade rhodamine B and generate electricity. With visible light irritation, the maximum photocurrent density, maximum power density, and degradation rate of the PFC were 0.59 mA cm−2, 29.88 μW cm−2, and 97.48% (1 h), respectively. The major active species in the PFC were h+, ˙O2−, and ˙OH. The good performance of the PFC was ascribed to the formation of a double Z-type heterojunction in the 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode so that the photoelectrons of NH2-MIL-125 and Bi2O3 directly combine with the photoholes of g-C3N4, making the photoholes of NH2-MIL-125 and Bi2O3 and the photoelectrons of g-C3N4 directly or indirectly involved in the RhB degradation process and generating electricity. Thus, the separation rate of the e−–h+ pairs in the photoanode and the capability of the PFC are greatly improved.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 15
·5815
·
IF 4.6
Dongmei Peng,Zhongfeng Zhang,Jijuan Zhang,Yang Yang
The photocatalytic degradation of formaldehyde by graphite-like C3N4is one of the most attractive and environmentally friendly strategies to address the significant threat to human health posed by indoor air pollutants. Despite its potential, this degradation process still faces issues with suboptimal efficiency, which may be attributed to the rapid recombination of photogenerated excitons and the broad band gap. As a proof of concept, a series of graphite-like C3N4@C60composites combining graphite-like C3N4and C60was developed via an in situ generation strategy. The obtained graphite-like C3N4@C60composites exhibited a remarkable increase in the photocatalytic degradation efficiency of formaldehyde, of up to 99%, under visible light irradiation, outperforming pure graphite-like C3N4and C60. This may be due to the composites’ enhanced built-in electric field. Additionally, the proposed composites maintained a formaldehyde removal efficiency of 84% even after six cycles, highlighting their potential for indoor air purification and paving the way for the development of efficient photocatalysts.Keywords:graphite-like C3N4/C60composite;robust built-in electric field;charge transfer;photocatalysis;formaldehyde degradation
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）